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Journal article

Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets

Kuhn T, Earle M, Khalizov A, Sloan J...(+4 more)

Atmospheric Chemistry and Physics, vol. 11, issue 6 (2011) pp. 2853-2861

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The relative roles of volume and surface nucleation were investigated
for the homogeneous freezing of pure water droplets. Experiments were
carried out in a cryogenic laminar aerosol flow tube using supercooled
water aerosols with maximum volume densities at radii between 1 and 3
mu m. Temperature- and size-dependent values of volume- and
surface-based homogeneous nucleation rates between 234.8 and 236.2 K
were derived using a microphysical model and aerosol phase compositions
and size distributions determined from infrared extinction measurements
in the flow tube. The results show that the contribution from
nucleation at the droplet surface increases with decreasing droplet
radius and dominates over nucleation in the bulk droplet volume for
droplets with radii smaller than approximately 5 mu m. This is
interpreted in terms of a lowered free energy of ice germ formation in
the surface-based process. The implications of surface nucleation for
the parameterization of homogeneous ice nucleation in numerical models
are considered.

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